In substituted calix[4]-arenes-cyclophanes consisting of four phenol m
oieties connected by methylene bridges-the number and also the relativ
e positions of the donor and/or acceptor pi-conjugated (D-pi-A) units
can be varied by changing the configuration. The Figure illustrates th
e cone configuration. The molecular and thin-film NLO properties of th
ree tetra-D-pi-A-substituted calix[4]arenes, including their orientati
on in thin films and the stability of their NLO properties, are descri
bed.